A compact expression is derived for the part of the cross section for light scattering by axisymmetrically polarized atomic systems proportional to the third-rank state multipole. The effect of the second-order orientation determined by this state multipole on the polarization and angular distribution of the scattered light is studied. The polarization of the incident light can be arbitrary and is specified by the Stokes parameters. A number of orientation effects in the scattering process are shown to be induced precisely by the second-order orientation. In particular, when nonpolarized light is scattered by an oriented atom, the scattering intensity in the perpendicular direction depends on the second-order orientation alone. The second-order orientation also preserves circular dichroism in the linear polarization of the forward-and back-scattered light.
A compact expression is derived for the part of the cross section for light scattering by axisymmetrically polarized atomic systems proportional to the third-rank state multipole. The effect of the second-order orientation determined by this state multipole on the polarization and angular distribution of the scattered light is studied. The polarization of the incident light can be arbitrary and is specified by the Stokes parameters. A number of orientation effects in the scattering process are shown to be induced precisely by the second-order orientation. In particular, when nonpolarized light is scattered by an oriented atom, the scattering intensity in the perpendicular direction depends on the second-order orientation alone. The second-order orientation also preserves circular dichroism in the linear polarization of the forward-and back-scattered light.
An expression for the cross section of light scattering by axisymmetrically aligned atomic systems is derived in a compact form. The cross section under consideration is proportional to the state multipole of the fourth rank. The effect of the second-order alignment determined by the fourth-rank state multipole on the polarization and the angular distribution of scattered light is investigated. The polarization of incident light can be arbitrary and, in the general case, is specified by the Stokes parameters. In particular, it is demonstrated that the second-order alignment cannot induce circular polarization of scattered light and does not influence the dissipation-induced effects of circular dichroism associated with the first-order alignment but leads to a change in the angular distribution and the degree of linear polarization of the scattered light.
A compact expression is derived for the cross section of scattering of arbitrarily polarized light by oriented atomic systems, in which the dependence on the geometric parameters and on the Stokes parameters preassigning the state of partial polarization of incident radiation is explicitly separated. It is found that the cross section of any photoprocess accompanied by photon absorption (stimulated emission) contains the sum of the products of the circular and linear dichroisms of the process by the respective Stokes parameters. The effect of the atomic orientation and of the dissipation of light energy on the polarization singularities and angular distribution of scattered light is investigated. In particular, it is demonstrated that, in the case of an open dissipation channel, the angular distribution remains dependent on the atomic orientation even in the case of zero degree of circular polarization of scattered radiation.
A compact expression for the cross section of scattering of an arbitrarily polarized light by aligned atomic systems is obtained, in which the dependence on the geometric parameters and the Stokes parameters specifying the state of partial polarization of the incident radiation is represented in explicit form. The effect of atomic alignment and the processes of dissipation of the light energy on the polarization specific features and the angular distribution of the scattered light is investigated. In particular, it is shown that, if a dissipative channel is accessible, the angular distribution and the degree of linear polarization of scattered light depend on the degree of circular polarization of the incident radiation η 2 . Dissipative processes also induce the circular polarization of the light scattered by aligned atoms when η 2 =0.
It is shown that new effects in light scattering by oriented atoms and in orientation of an unpolarized atomic target due to the light scattering arise when channels of dissipation for the light energy are open. Thus, in scattering of linearly-polarized or unpolarized light, the degree of linear polarization and the angular distribution of scattered light depend on the initial atomic orientation. On the other hand, the orientation of unpolarized atoms appears in the scattering of unpolarized photons without registration of the scattered photon polarization. The orientation vector is perpendicular to the scattering plane, and the effect can be observed in a coincidence experiment.
The theory of optical birefringence is discussed from the point of view of the scattering of polarized photons by molecules using the framework of formal scattering theory and quantum electrodynamics. In Part One, those features from noncovariant quantum electrodynamics relevant to the molecular scattering of photons are reviewed. Chapter One contains an outline of classical electrodynamics in the Coulomb gauge, including the Stokes parameter and density matrix formulations of polarization. Chapter Two deals with the quantization of the radiation field, and the occupation number representation is defined. The quantum mechanical description of polarized light is outlined in Chapter Three: operator equivalents of the density matrix and Stokes parameters are invoked, the parameters themselves being obtained from the expectation values of the Stokes operators with the state vector of the photon. The Stokes parameter and density matrix are then applied to the polarization of a general beam containing an arbitrary number of photons, and some new methods are developed. The interaction of the electromagnetic field with bound electrons is formulated in Chapter Four in terms of a canonically transformed interaction Hamiltonian in which the multipole terms are explicit. Since each term is then gauge-invariant, this Hamiltonian is particularly suited to the application of diagrammatic perturbation theory which follows from the iteration of the scattering matrix in the interaction representation (Chapter Five). Also the extension of the theory to multiphoton processes is facilitated "because the field strength is explicit in the transformed Hamiltonian. The S-matrix connects the initial and final asymptotic states of the scattering system, and in Chapter Six the state vector and density operator of the scattered photon beam are obtained from those of the incident beam. Part Two contains the application of the above methods to a variety of linear and nonlinear optical birefringence effects in the absence or presence of external fields. In Chapter Seven, general equations are obtained for the polarization changes imposed on a forward scattered photon in terms of matrix elements of the reaction operator between plane polarized photon base states; whereas Chapter Eight extends this treatment to an n-photon beam, thereby encompassing the hyperpolarizability contributions to the polarization changes of the forward scattered beam. It is then demonstrated that the fundamental process in optical birefringence can be interpreted as an infinitesimal unitary transformation of the polarization spinor. Also the S-matrix approach to birefringence is compared with the methods used in crystal optics, and with the classical treatments of the scattering of polarized light by molecules. The general equations obtained for the polarization changes of the forward scattered beam are subsequently interpreted in the light of the physical circumstances appropriate to the bire- fringence effect of interest. In Chapters Nine, Ten, and Eleven, diagrammatic perturbation theory is used to obtain explicit expressions, in terms of molecular polarizability and rotation tensors, for the linear and nonlinear contributions to the polarization changes involved in natural optical activity, and in birefringence phenomena induced by static and optical electric and magnetic fields. The nonforward scattering of polarized photons by molecules is discussed in Part Three. General equations are calculated in Chapter Twelve for the azimuth, ellipticity, and depolarization ratio of the Rayleigh beam at any scattering angle and for any polarization of the incident beam. Explicit expressions in terms of molecular quantities are then obtained for the polarization at scattering angles of 90° and almost zero from both optically inactive and optically active molecules. It is demonstrated that a determination of the precise polarization state of the scattered beam can provide useful molecular information additional to that obtained from depolarization ratios alone. This is because the depolarization ratio depends on only the diagonal elements of the polarization density matrix and so does not convey all the information about the system. Raman scattering processes are contained in the formulation and the polarization of the Raman light at any scattering angle can be obtained. This is shown to be particularly useful for predicting the polarization of stimulated Raman light for any Raman-active liquid placed within a laser cavity. By extending the nonforward scattering formulation to incorporate multiphoton processes, equations are obtained in Chapter Thirteen for the ellipticity, azimuth, and depolarization ratio of the second harmonic wave at any scattering angle as a function of the incident polarization. Several specific situations are subsequently investigated. Finally, it is shown in Chapter Fourteen that the near-forw- ard Rayleigh and Raman scattering formulations provide an explanation for the observed polarization, as a function of the initial polarization, of the self-trapped filaments that arise from the self-focusing of an intense laser beam.
Using the electric dipole approximation, we present, in invariant form, the cross section of an arbitrary three-photon transition between the discrete states of an atom with total angular momenta J i and J f . The cross section contains scalar and mixed products of the photon polarization vectors, and invariant atomic parameters dependent only on the photon frequencies. We determine the number of independent atomic parameters at fixed values of J i and J f and obtain their explicit expressions in terms of the reduced composite dipole matrix elements. The polarization dependence of the cross sections is expressed in terms of the degrees l and ξ of linear and circular photon polarizations. We analyze the phenomenon of dissipation-induced circular dichroism in three-photon processes, i.e., the difference Δ of the cross sections for opposite signs of the degree of circular polarization of all the photons. We study in detail the case of two identical photons and the phenomenon of elliptical dichroism, when Δ∼ lξ holds and dichroism occurs only when the photons are elliptically polarized, with 0<| ξ |<1. Finally, we discuss the dissipation-induced effects of atom polarization in three-photon processes involving linearly polarized or unpolarized photons.